CN111755664B - Electrode of lithium ion battery and lithium ion battery - Google Patents
Electrode of lithium ion battery and lithium ion battery Download PDFInfo
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- CN111755664B CN111755664B CN202010620634.2A CN202010620634A CN111755664B CN 111755664 B CN111755664 B CN 111755664B CN 202010620634 A CN202010620634 A CN 202010620634A CN 111755664 B CN111755664 B CN 111755664B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The present disclosure relates to an electrode of a lithium ion battery and a lithium ion battery, the electrode includes a current collector and an active material layer stacked on the surface of the current collector, the active material layer contains an electrode active material and a first lithium salt, the first lithium salt accounts for the content of the active material layer is not more than 10 wt%, and the active material layer has a concentration gradient that the concentration of the first lithium salt decreases along a direction away from the current collector. According to the lithium ion battery containing the electrode, especially the lithium ion power battery, the lost lithium salt can be supplemented in time in the using process, the constant conductivity of the lithium ion in the electrolyte is kept, and therefore the power attenuation of the lithium ion battery in the whole life cycle of the battery is reduced.
Description
Technical Field
The present disclosure relates to the technical field of lithium ion batteries, and particularly, to an electrode of a lithium ion battery and a lithium ion battery.
Background
The lithium ion power battery is a novel high-energy battery successfully developed in the 20 th century. The negative electrode of the battery is usually graphite, and the positive electrode is usually lithium iron phosphate, lithium cobaltate and lithium titanate. The lithium ion power battery has the advantages of high energy, high battery voltage, wide working temperature range and long storage life, and is widely applied to military and civil small-sized electrical appliances. For lithium ion power batteries, it is desirable to have good power retention capability. The power maintenance of the power battery directly affects the acceleration performance and the charging capability of the electric vehicle in the whole life cycle, so the power maintenance performance of the power battery is required to be higher and higher. The power requirement is not only at the initial stage of the service life, but also is very important for the whole service life cycle of the electric vehicle, the electric vehicle is required to have good acceleration performance and charging capacity in the whole service life cycle, and the problem of overlarge attenuation cannot be caused relative to the initial stage.
In the prior art, methods for improving the power retention performance of a lithium ion power battery include the following three methods: cathode side: particle size reduction or surface coating; in the aspect of an anode: particle size reduction or surface functional group modification; electrolyte aspect: adding a film stabilizer or increasing the lithium salt concentration. The disadvantages are as follows: in the cathode aspect: the specific capacity of the particles is exerted due to the reduction of the particle size or the surface coating, the compaction density is reduced due to the surface coating or the size reduction, the energy density of the battery cell is further deteriorated, and on the other hand, the specific surface area is increased due to the size reduction, so that the long-term storage performance of the battery cell is deteriorated; in the aspect of an anode: the specific capacity of the deteriorated particles is exerted by reducing the particle size or modifying the surface functional groups, meanwhile, the compaction density is reduced by coating or reducing the size on the surface, the first efficiency of the material is reduced by modifying the surface functional groups, the consumption of active lithium is increased, the energy density of the battery core is further deteriorated, and on the other hand, the specific surface area is increased by reducing the size, and the long-term storage performance of the battery core is deteriorated; electrolyte aspect: the addition of the membrane stabilizer stabilizes the surface structure of the electrode, increases the thickness of a solid-phase electrolyte membrane on the surface to a certain extent, increases the membrane impedance and deteriorates the initial power performance; increasing the lithium salt concentration ensures electrolyte conductivity throughout the life, but increases the initial electrolyte viscosity, leading to deterioration of initial power performance, especially low temperature performance.
Disclosure of Invention
In order to overcome the defects of the prior art and improve the power holding capacity of the lithium ion battery, the disclosure provides an electrode of the lithium ion battery and the lithium ion battery.
In order to achieve the above object, a first aspect of the present disclosure provides an electrode for a lithium ion battery, the electrode including a current collector and an active material layer laminated on a surface of the current collector, the active material layer containing therein an electrode active material and a first lithium salt, the first lithium salt accounting for not more than 10 wt% of the active material layer, the active material layer having a concentration gradient in which a concentration of the first lithium salt decreases in a direction away from the current collector.
Optionally, the active material layer comprises a plurality of active material sublayers stacked, and the concentration of the first lithium salt in the active material sublayers decreases in a direction away from the current collector; wherein, in the active material sub-layer farthest from the current collector, the content of the first lithium salt is 0 to 2 wt%.
Optionally, the number of the plurality of active material sublayers is 2 to 6.
Optionally, the number of the active material sublayers is 2; the content of the first lithium salt in the active material sub-layer closest to the current collector is 1-5 wt%, and the content of the first lithium salt in the active material sub-layer farthest from the current collector is 0-2 wt%;
preferably, in the active material sub-layer closest to the current collector, the content of the first lithium salt is 2 to 4 wt%, and in the active material sub-layer farthest from the current collector, the content of the first lithium salt is 0 to 1 wt%.
Optionally, the active material layer has a thickness of 30 to 300 μm; the thickness of the single active material sublayer accounts for 5-95% based on the thickness of the active material layer.
Optionally, the first lithium salt comprises LiPF 6 、LiClO 4 、LiBO 2 、LiAsF 6 And LiBF 4 One or more of the above; the current collector is selected from aluminum foil and/or copper foil;
the electrode is an anode, the active substance layer contains an anode active substance, and the anode active substance comprises one or more of natural graphite, artificial graphite, soft carbon, hard carbon and silicon alloy; alternatively, the first and second electrodes may be,
the electrode is a cathode, the active material layer contains a cathode active material, and the cathode active material comprises LiNi x Co y Mn z 、LiFe a Al b P c O 4 Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is equal to 1; a is more than or equal to 0 and less than or equal to 1, b is more than or equal to 0 and less than or equal to 0.8, c is more than or equal to 0 and less than or equal to 2, and a + b + c is equal to 2.
A second aspect of the present disclosure provides a lithium ion power cell comprising an electrode according to the first aspect of the present disclosure.
Optionally, the anode and/or the cathode of the lithium ion battery is/are the electrode of any one of claims 1 to 6, and the lithium ion battery further comprises a separator and an electrolyte.
Optionally, the diaphragm is one or more of a polyethylene diaphragm, a polypropylene diaphragm and a non-woven fabric diaphragm;
the electrolyte contains a second solvent and a second lithium salt; the second solvent comprises a cyclic ester and/or a linear ester; preferably, the second solvent is one or more of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate and ethyl methyl carbonate; the second lithium salt is LiPF 6 、LiClO 4 、 LiBO 2 、LiAsF 6 And LiBF 4 One or more of them.
Optionally, the lithium ion battery is a lithium ion power battery.
The electrode comprises an electrode current collector and an active material layer arranged on the surface of the electrode current collector, wherein the active material layer contains lithium salt, the concentration of the lithium salt is reduced along the gradient of the direction far away from the current collector, the electrode can timely and continuously supplement the lithium salt loss in electrolyte in the using process, the conductivity of lithium ion in the electrolyte is kept stable, and the power attenuation of a lithium ion battery containing the electrode, especially a lithium ion power battery in the whole service life cycle of the battery can be obviously reduced.
Additional features and advantages of the present disclosure will be set forth in the detailed description which follows.
Detailed Description
Specific embodiments of the present disclosure are described in detail below. It should be understood that the detailed description and specific examples, while indicating the present disclosure, are given by way of illustration and explanation only, and are not intended to limit the present disclosure.
The first aspect of the present disclosure provides an electrode of a lithium ion battery, the electrode including a current collector and an active material layer laminated on a surface of the current collector, the active material layer containing therein an electrode active material and a first lithium salt, the first lithium salt constituting not more than 10 wt% of the active material layer, the active material layer having a concentration gradient in which a concentration of the first lithium salt decreases in a direction away from the current collector.
The electrode comprises an electrode current collector and an active material layer arranged on the surface of the electrode current collector, wherein the active material layer contains lithium salt, the concentration of the lithium salt is reduced along the gradient of the direction far away from the current collector, the electrode can timely and continuously supplement the lithium salt loss in electrolyte in the using process, the conductivity of lithium ion in the electrolyte is kept stable, and the power attenuation of a lithium ion battery containing the electrode, especially a lithium ion power battery in the whole service life cycle of the battery can be obviously reduced.
According to the present disclosure, the active material layer having a concentration gradient in which the concentration of the first lithium salt decreases in a direction away from the current collector means: in the active material layer, the concentration of the first lithium salt increases or does not change as the distance from the surface of the current collector increases. For example, in the active material layer, the concentration of the first lithium salt may be continuously decreased or stepwise decreased in a direction away from the current collector.
In one embodiment, the active material layer may include a plurality of active material sublayers stacked in a thickness direction, and the concentration of the first lithium salt in each active material sublayer decreases in a direction away from the current collector, wherein the concentration of the first lithium salt in each active material sublayer refers to an average concentration of the first lithium salt in the active material sublayer.
In one embodiment, the number of active material sublayers is 2 to 6, and preferably may be 2 to 4.
According to the present disclosure, the content of the first lithium salt in the active material layer may be not more than 10% by weight, for example, 0.01 to 10%, 0.1 to 10%, 0.2 to 9.8%, or 0.5 to 9.5% by weight, in order to continuously and smoothly replenish the lithium salt into the electrolyte during long-term cyclic charge and discharge while maintaining the overall capacity and energy density of the electrode. In a further embodiment, the first lithium salt is present in an amount of no more than 8 wt%, such as 0.1-8 wt%, 0.2-8 wt%, 0.5-7.8 wt%, or 1-7.5 wt%, based on the total weight of the active material layer.
In order to further smoothly release the first lithium salt into the electrolyte, in one embodiment of the present disclosure, in the active material sublayer farthest from the current collector, the content of the first lithium salt may be 0 to 2 wt%, and preferably may be 0.5 to 1.5 wt%, so as to avoid that the lithium salt content in the electrolyte is too high, the viscosity is increased, and the initial power performance of the lithium ion battery is reduced.
In the embodiment where the active material layer includes a plurality of active material sublayers, the number of the active material sublayers is not particularly limited, and may be, for example, 2 to 20, 2 to 10, or 2 to 8, and in a preferred embodiment, the number of the plurality of active material sublayers is 2, wherein, in the active material proton layer closest to the current collector, the content of the first lithium salt may be 1 to 5 wt%, and in the active material sublayer farthest from the current collector, the content of the first lithium salt may be 0 to 2 wt%; in a further preferred embodiment, the content of the first lithium salt in the active material sublayer closest to the current collector may be 2 to 4 wt%, and the content of the first lithium salt in the active material sublayer farthest from the current collector may be 0 to 1 wt%.
According to the present disclosure, the thickness of the active material layer is not particularly limited, and in one embodiment, the thickness of the active material layer may be 30 to 300 μm, and preferably may be 50 to 260 μm; in a further embodiment, the thickness of the individual active substance sublayers may be from 5 to 95%, preferably from 10 to 80%, based on the thickness of the active substance layer.
The present disclosure is not limited with respect to the type of first lithium salt in the active material sublayer, and may be a conventional choice for the present disclosure, and in one embodiment, the first lithium salt may comprise LiPF 6 、LiClO 4 、LiBO 2 、 LiAsF 6 And LiBF 4 Preferably, it may be LiPF 6 、LiClO 4 And LiBO 2 One or more of them.
According to the present disclosure, the active material layer of the electrode may further include one or more of a conductive agent, a binder, and a thickener, and the types and contents of the conductive agent, the binder, and the thickener may be conventional in the art and are not described herein again.
The electrode of the lithium ion power battery of the present disclosure may be an anode and/or a cathode, the present disclosure is not limited, in one embodiment, the electrode may be an anode, the active material layer contains an anode active material, the anode active material may include one or more of natural graphite, artificial graphite, soft carbon, hard carbon and a silicon alloy, preferably, the anode active material may include one or more of natural graphite, hard carbon and a silicon alloy, and the current collector of the anode may be selected from an aluminum foil or a copper foil.
In another embodiment, the electrode may be a cathode, the active material layer may contain a cathode active material, and the anode active material may include LiNi x Co y Mn z 、LiFe a Al b P c O 4 Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is equal to 1; a is more than or equal to 0 and less than or equal to 1, b is more than or equal to 0 and less than or equal to 0.8, c is more than or equal to 0 and less than or equal to 2, and a + b + c is 2; the current collector of the cathode may be selected from aluminum foil or copper foil.
In one embodiment, the electrode of the lithium ion power battery of the present disclosure may be prepared by: mixing the first lithium salt with different contents with an electrode active material and a first solvent respectively to prepare slurry containing the first lithium salt with different concentrations; coating the slurry containing the first lithium salt with different concentrations on the surface of a current collector; and then drying, rolling, die cutting and punching to obtain the electrode plate.
The first solvent for formulating the slurry in the present disclosure is not limited and may be a conventional choice in the art, for example, may be one or more of N-methylpyrrolidone, dimethylformamide, methyl acetate and tetrahydrofuran.
The present disclosure is not limited to the manner of coating the slurry on the surface of the current collector, and may be a routine operation in the field, for example, multiple slurries containing different concentrations of the first lithium salt may be prepared, and the multiple slurries may be coated on the current collector to form multiple active material layers having a concentration gradient in which the concentration of the first lithium salt decreases in a direction away from the current collector.
In one embodiment, the multiple slurries containing the first lithium salts with different concentrations are introduced into a multi-cavity coater with a plurality of stacked different cavities according to the arrangement that the concentrations of the first lithium salts are gradually decreased from bottom to top, and all the slurries with different concentrations are distributed on the current collector at one time; in a more specific embodiment, two chambers (referred to as an upper chamber and a lower chamber, respectively) are filled with slurries with different first lithium salt concentrations, specifically, the slurry with the smaller first lithium salt concentration is filled in the upper chamber, the slurry with the higher first lithium salt concentration is filled in the lower chamber, and outlets of the upper chamber and the lower chamber are opened simultaneously to perform primary coating, so that the upper chamber slurry and the lower chamber slurry are distributed on the surface of the current collector in a stacked manner, after the solvent is removed, a pole piece with two active material sub-layers is formed, and the first lithium salt concentration in an upper active material proton layer far away from the current collector is low, and the first lithium salt concentration in a lower active material sub-layer close to the current collector is high.
In another embodiment, slurries containing different concentrations of the first lithium salt may be sequentially coated on the surface of the current collector in the order of the concentration of the first lithium salt from large to small, for example, multiple times by a single-chamber coater; optionally, a step of drying to remove the first solvent may be performed between the two coating.
A second aspect of the present disclosure provides a lithium ion battery, in particular a lithium ion power battery, comprising an electrode according to the first aspect of the present disclosure.
The lithium ion battery disclosed by the invention adopts the electrode disclosed by the invention, lithium salt can be stably and continuously supplemented to the electrolyte in the battery cycle process, and the constant of the lithium ion conductivity in the electrolyte is kept, so that the power attenuation of the lithium ion battery in the whole battery life cycle is reduced.
According to an embodiment of the present disclosure, the anode of the lithium ion battery is the electrode according to the first aspect of the present disclosure; in another embodiment, the cathode of the lithium ion battery is the electrode according to the first aspect of the present disclosure; in a third embodiment, the cathode and the anode of the lithium ion battery are the electrodes according to the first aspect of the present disclosure, respectively.
In a further embodiment, the lithium ion battery further comprises a separator and an electrolyte.
According to the present disclosure, the separator of the lithium ion power battery may be of a kind conventional in the art, and for example, may be one or more of a polyethylene separator, a polypropylene separator, and a non-woven fabric separator, and preferably may be one or more of a polyethylene separator and a non-woven fabric separator.
According to the present disclosure, lithium ion mobilityThe composition of the electrolyte of the power cell may be conventional in the art, for example, the electrolyte may contain a second solvent and a second lithium salt; the second lithium salt may be the same as or different from the first lithium salt. In one embodiment, the second solvent may include cyclic ester and/or linear ester, and preferably, the second solvent may be one or more of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate and ethyl methyl carbonate, and more preferably, may be one or more of polyethylene carbonate, propylene carbonate and ethyl methyl carbonate; in a further embodiment, the second lithium salt may be LiPF 6 、 LiClO 4 、LiBO 2 、LiAsF 6 And LiBF 4 Preferably, it may be LiPF 6 、LiClO 4 And LiBO 2 One or more of them.
The present disclosure is further illustrated by the following examples, but is not to be construed as being limited thereby.
LiNi was used as a cathode active material in each of the following examples and comparative examples 0.5 Co 0.2 Mn 0.3 O 2 The cathode current collector is an aluminum foil with the thickness of 12 mu m; the anode active substances are all made of artificial graphite materials, and the anode current collector is a copper foil with the thickness of 8 mu m; the diaphragms are polyethylene PE diaphragms with the thickness of 16 mu m; the electrolyte adopts LiPF containing 1.12M 6 Lithium salt and a solvent (diethyl carbonate DEC: ethylene carbonate EC: ethyl methyl carbonate EMC: 1: 1).
Example 1
In this example, the separator of the lithium ion power battery is a Polyethylene (PE) separator with a thickness of 12 μm, the second solvent in the electrolyte is ethylene carbonate/ethyl methyl carbonate (volume ratio 5: 5), and the second lithium salt is LiPF 6 The cathode has a single layer of active material, and the anode has 2 active material sublayers; the preparation method of the anode comprises the following steps:
homogenizing anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose) and SP (conductive agent) according to a weight ratio of 95:2.5:1.5:1, adding water to control the solid content to be 45-55%, and controlling the viscosity to be 2000-4000 mpa.s, and introducing the anode slurry into an upper cavity after stirring;
taking anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion Polymer) 6 Homogenizing (first lithium salt) according to a weight ratio of 94:2.5:1.5:1:1, wherein water is added to control the solid content to be 45-55%, and the viscosity is 2000-4000mpa · s, and after stirring is finished, introducing anode slurry into a lower cavity;
uniformly coating the upper cavity slurry and the lower cavity slurry on the surface of a copper foil with the thickness of 8 mu m, wherein the coating weight of the two surfaces of the copper foil is 181g/m 2 The upper layer coating weight is controlled to be 90.5g/m by controlling the upper cavity gasket and the lower cavity gasket and the clamping degree 2 The lower layer coating weight was 90.5g/m 2 And then drying, rolling, die cutting and punching to obtain the anode plate. Wherein the total thickness of the active material layer is 120 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 5: 5.
example 2
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the preparation of slurry introduced into the lower cavity, anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion power) are taken 6 (lithium salt) was homogenized at a weight ratio of 93:2.5:1.5:1: 2.
Example 3
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the preparation of slurry introduced into the lower cavity, anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion power) are taken 6 (lithium salt) was homogenized at a weight ratio of 92:2.5:1.5:1: 3.
Example 4
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the preparation of slurry introduced into the lower cavity, anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion power) are taken 6 (lithium salt) was homogenized at a weight ratio of 91:2.5:1.5:1: 4.
Example 5
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the preparation of slurry introduced into the lower cavity, anode graphite and SBR (styrene butadiene rubber) are taken,CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF 6 (lithium salt) was homogenized at a weight ratio of 90:2.5:1.5:1: 5.
Example 6
A lithium ion power cell was prepared using the method of example 1, with the only difference that: during the preparation of the slurry introduced into the upper cavity, the anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion phosphate) are taken 6 (lithium salt) homogenizing according to a weight ratio of 94:2.5:1.5:1: 1;
in the preparation of slurry introduced into the lower cavity, anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethyl cellulose), SP (conductive agent) and LiPF (lithium ion power) are taken 6 (lithium salt) is homogenized according to the weight ratio of 93:2.5:1.5:1: 2.
Example 7
A lithium ion power cell was prepared using the method of example 1, except that: the anode has a single active material layer, and the cathode has 2 active material sublayers; the preparation method of the cathode comprises the following steps:
taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Homogenizing according to the weight ratio of NCM (ternary material), PVDF (polyvinylidene fluoride) and SP (conductive agent) of 95:3:2, wherein NMP (N-methyl-2 pyrrolidone) is added to control the solid content to be 68-75%, the viscosity is 6000-10000mpa & s, and after stirring, the cathode slurry is introduced into an upper cavity;
cathode taking LiNi 0.5 Co 0.2 Mn 0.3 O 2 The ternary material is homogenized according to the weight ratio of NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent) and LiPF6 (lithium salt) of 94:3:2:1, wherein NMP (N methyl-2 pyrrolidone) is added to control the solid content to be 68-75%, and the viscosity is 6000-10000mpa & s. After stirring is completed, the cathode slurry is introduced into the lower cavity;
the slurry of the upper cavity and the lower cavity is evenly coated on the surface of a 12 mu m aluminum foil substrate, and the coating weight of the two surfaces is 381g/m 2 The upper layer coating weight is controlled to be 190.5g/m by controlling the upper cavity gasket and the lower cavity gasket and the clamping degree 2 The lower layer coating weight was 190.5g/m 2 And then the cathode plate is obtained by drying, rolling, die cutting and punching. Wherein the total thickness of the active material layerThe degree is 140 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 5: 5.
example 8
A lithium ion power cell was prepared using the method of example 8, except that: in the preparation of slurry introduced into the lower cavity, taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Ternary materials, such as NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF (conductive polymer) 6 The homogenization was performed at a weight ratio of (lithium salt) 93:3:2: 2.
Example 9
A lithium ion power cell was prepared using the method of example 8, except that: in the preparation of slurry introduced into the lower cavity, a cathode LiNi is taken 0.5 Co 0.2 Mn 0.3 O 2 Ternary materials, such as NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF (conductive polymer) 6 Homogenization was performed at a weight ratio of (lithium salt) 92:3:2: 3.
Example 10
A lithium ion power cell was prepared using the method of example 8, except that: in the preparation of slurry introduced into the lower cavity, taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Ternary materials, such as NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF 6 Homogenization was performed at a ratio of (lithium salt) 91:3:2:4 by weight.
Example 11
A lithium ion power cell was prepared using the method of example 8, with the only difference that: in the preparation of slurry introduced into the lower cavity, a cathode LiNi is taken 0.5 Co 0.2 Mn 0.3 O 2 Ternary materials, such as NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF (conductive polymer) 6 Homogenization was performed at a ratio of (lithium salt) ═ 90:3:2:5 by weight.
Example 12
A lithium ion power cell was prepared using the method of example 8, with the only difference that: during the preparation of the slurry introduced into the upper cavity, taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Ternary materials, such as NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF (conductive polymer) 6 (lithium salt) at a weight ratio of 94:3:2: 1;
in the preparation of slurry introduced into the lower cavity, a cathode LiNi is taken 0.5 Co 0.2 Mn 0.3 O 2 Ternary material, according to NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF 6 The homogenization was performed at a weight ratio of (lithium salt) 93:3:2: 2.
Example 13
A lithium ion power cell was prepared using the method of example 1, except that: the anode has 2 active material sublayers, and the cathode has 2 active material sublayers;
the preparation method of the cathode comprises the following steps:
taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Ternary material, according to NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent), LiPF 6 Homogenizing at a weight ratio of 94:3:2:1, adding NMP (N-methyl-2-pyrrolidone) to control the solid content to be 68-75%, and controlling the viscosity to be 6000-10000mpa & s, and after stirring, introducing cathode slurry into an upper cavity;
taking cathode LiNi 0.5 Co 0.2 Mn 0.3 O 2 Ternary material, according to NCM (ternary material), PVDF (polyvinylidene fluoride), SP (conductive agent) LiPF 6 Homogenizing at a weight ratio of 93:3:2:2 of (lithium salt), adding NMP (N-methyl-2-pyrrolidone) to control the solid content to be 68-75% and the viscosity to be 6000-10000mpa & s, and introducing the cathode slurry into a lower cavity after stirring;
the upper cavity slurry and the lower cavity slurry are evenly coated on the surface of an aluminum foil substrate with the thickness of 12 mu m, and the coating weight of the two surfaces is 383g/m 2 The upper layer coating weight is controlled to be 191.5g/m by controlling the upper cavity gasket and the lower cavity gasket and the clamping degree 2 The lower layer coating weight was 191.5g/m 2 And then drying, rolling, die cutting and punching to obtain the cathode plate. Wherein the total thickness of the active material layer is 142 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 5: 5.
the preparation method of the anode comprises the following steps:
taking anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium iron phosphate) 6 (lithium salt) was homogenized at a weight ratio of 94:2.5:1.5:1:1, wherein water was added to control the solid content to 45-55%, viscosity 2000-4000mpa · s. After the stirring is completed, the anode slurry is introduced into the upper chamber.
Taking anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion phosphate) 6 (lithium salt) was homogenized at a weight ratio of 93:2.5:1.5:1:2, wherein water was added to control the solid content to 45-55%, viscosity 2000-4000mpa · s. After the stirring is completed, the anode slurry is introduced into the lower cavity.
The upper cavity slurry and the lower cavity slurry are uniformly coated on the surface of a copper foil substrate with the thickness of 8 mu m, and the coating weight of the two surfaces is 183g/m 2 The upper layer coating weight is controlled to be 91.5g/m by controlling the upper cavity gasket and the lower cavity gasket and the clamping degree 2 The lower layer coating weight was 91.5g/m 2 And then drying, rolling, die cutting and punching to obtain the anode plate. Wherein the total thickness of the active material layer is 122 μm, and the thickness ratio of the upper active material sublayer to the lower active material proton layer is 5: 5.
example 14
A lithium ion power cell was prepared using the method of example 15, except that: during the preparation of the anode, the coating weight of the upper layer was 54.9g/m 2 The lower layer coating weight was 128.1g/m 2 . Wherein the total thickness of the active material layer is 122 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 3: 7.
example 15
A lithium ion power cell was prepared using the method of example 15, with the only difference that: during the preparation of the anode, the coating weight of the upper layer is 128.1g/m 2 The lower layer coating weight was 54.9g/m 2 . Wherein the total thickness of the active material layer is 122 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 7: 3.
example 16
A lithium ion power cell was prepared using the method of example 15, except that: during the preparation of the cathode, the upper layer coating weight was 114.9g/m 2 The lower layer coating weight was 268.1g/m 2 . Wherein the total thickness of the active material layerThe degree is 142 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 3: 7.
example 17
A lithium ion power cell was prepared using the method of example 15, except that: during the preparation of the cathode, the upper coating weight was 268.1g/m 2 . Wherein the total thickness of the active material layer is 142 μm, and the thickness ratio of the upper active material sublayer to the lower active material sublayer is 3: 7.
example 18
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the upper active material sublayer of the anode, LiPF 6 The content of the (first lithium salt) was 3 wt%, and the anode graphite was homogenized with SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose) and SP (conductive agent) in a weight ratio of 93:2.5:1.5: 3.
Example 19
A lithium ion power cell was prepared using the method of example 1, with the only difference that: the number of the active material sublayers is 8, the total thickness of the active material sublayers is 400 mu m, and the thickness of each active material proton layer is the same.
Example 20
A lithium ion power cell was prepared using the method of example 1, with the only difference that: in the lower active material sublayer close to the current collector, the content of the first lithium salt is 6 wt%, and anode graphite is homogenized with SBR (butadiene styrene rubber), CMC (sodium carboxymethylcellulose) and SP (conductive agent) according to the weight ratio of 90:2.5:1.5: 6; in an upper active material sublayer far away from the current collector, the content of the first lithium salt is 3 wt%, and anode graphite is homogenized with SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose) and SP (conductive agent) according to a weight ratio of 93:2.5:1.5: 3.
Comparative example 1
A lithium ion power cell was prepared using the method of example 1, with the only difference that: the active material layers of the anode and the cathode do not contain lithium salts.
Comparative example 2
A lithium ion power cell was prepared using the method of example 1, with the only difference that: the anode included only one active material layer having a thickness of 15 μm, the active material layer containing 0.5 wt% of lithium salt, with no concentration gradient.
Comparative example 3
A lithium ion power cell was prepared using the method of example 1, with the only difference that:
taking anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose) and SP (conductive agent) to homogenize according to the weight ratio of 85:2.5:1.5:1:10, adding water to control the solid content to be 45-55%, and controlling the viscosity to be 2000-4000 mpa.s, and introducing the anode slurry into an upper cavity after stirring;
taking anode graphite, SBR (styrene butadiene rubber), CMC (sodium carboxymethylcellulose), SP (conductive agent) and LiPF (lithium ion Polymer) 6 (first lithium salt) is homogenized according to the weight ratio of 80:2.5:1.5:1:15, wherein water is added to control the solid content to be 45-55%, the viscosity is 2000-4000mpa · s, and after stirring is finished, anode slurry is introduced into a lower cavity.
Test example 1
Taking the cathode pole piece and the anode pole piece in the embodiment and the comparative example, overlapping the pole pieces layer by layer in the order of the anode, the diaphragm, the cathode, the diaphragm and the anode to manufacture a naked battery cell, controlling the thickness of the naked battery cell to be consistent in the embodiment and the comparative example by controlling the number of the cathode and anode laminations, then putting the naked battery cell into a shell, baking, injecting liquid, forming, sealing and manufacturing the battery cell. The cell capacity, internal resistance and gravimetric energy density of the examples and comparative examples were tested separately and the results are shown in table 1. The specific operation is as follows:
at room temperature, three cells in each example and comparative example are taken, the cells are charged to 4.2V at constant current and constant voltage according to the charging 0.33C by adopting a charging and discharging test cabinet (model number BTS1000), the cells are discharged to 2.8V according to the discharging 0.33C after being placed for 10min, and the discharging capacity is recorded;
the cell impedances in the examples and comparative examples were tested with a resistance tester (model IT 5100);
the cell weights in the examples and comparative examples were measured using an electronic scale (model JTS-A), and the cell weight energy density is discharge capacity discharge plateau voltage/cell weight.
TABLE 1
From the cell capacity, impedance and energy density data of comparative examples and examples in table 1, it can be seen that, compared to comparative example 1, the addition of lithium salt to the electrodes in examples 1 to 20 results in a decrease in the content ratio of the active material in the electrode, and a decrease in the energy density per unit weight, resulting in a slight decrease in capacity, but the addition of lithium salt has substantially no effect on ohmic impedance; as can be seen from the comparison of the data of examples 1 to 17 with examples 18 and 20, in the case where the content of the lithium salt in the active material sub-layer farthest from the current collector is 0 to 2 wt% as preferred in the present disclosure, the capacity and energy density of the lithium ion battery can be maintained at a high level, and the phenomenon of viscosity increase, polarization increase, capacity exertion deterioration, etc. due to too early dissolution of the lithium salt in the electrolyte in this layer can be avoided.
Test example 2
At room temperature, 2 cells in the comparative example and the example are taken, constant-current constant-voltage charging is carried out to 4.2V by using 0.33C, standing is carried out for 5min, then discharging is carried out to 2.8V by using 0.33C, and the discharging capacity is recorded, wherein the capacity retention rate is corresponding to the cycle discharging capacity/initial discharging capacity. The process is repeated until the capacity retention rate is less than or equal to 80 percent, and the number of cycles is recorded.
At room temperature, 2 cells in each of comparative examples and examples were taken, charged to 4.2V with a constant current and a constant voltage of 0.33C, and then placed in a high-temperature 45 ℃ incubator, stored for 500 days, and the capacity retention ratio was measured every 30 days. The results are shown in Table 2.
TABLE 2
| Serial number | Number of cycles @ 80% SOH | Capacity retention @500D |
| Examples 1 to 1 | 2929 | 81.8 |
| Examples 1 to 2 | 2912 | 82.1 |
| Example 2-1 | 2943 | 82.2 |
| Examples 2 to 2 | 2937 | 82.5 |
| Example 3-1 | 2958 | 82.6 |
| Examples 3 to 2 | 2942 | 82.9 |
| Example 4-1 | 2973 | 83.0 |
| Example 4 to 2 | 2956 | 83.3 |
| Example 5-1 | 2918 | 81.5 |
| Examples 5 and 2 | 2921 | 81.8 |
| Example 6-1 | 2973 | 83.0 |
| Example 6 to 2 | 2944 | 83.3 |
| Example 7-1 | 2875 | 81.7 |
| Example 7-2 | 2895 | 81.9 |
| Example 8-1 | 2949 | 83.1 |
| Example 8 to 2 | 2940 | 83.3 |
| Example 9-1 | 2964 | 83.6 |
| Example 9-2 | 2924 | 83.7 |
| Example 10-1 | 2979 | 84.0 |
| Example 10-2 | 2939 | 84.1 |
| Example 11-1 | 2894 | 81.3 |
| Example 11-2 | 2853 | 81.6 |
| Example 12-1 | 2979 | 82.9 |
| Example 12-2 | 2939 | 83.2 |
| Example 13-1 | 3002 | 83.9 |
| Example 13-2 | 2986 | 84.2 |
| Example 14-1 | 2972 | 83.0 |
| Example 14-2 | 2956 | 83.3 |
| Example 15-1 | 2943 | 82.2 |
| Example 15-2 | 2926 | 82.5 |
| Example 16-1 | 2972 | 83.0 |
| Example 16-2 | 2956 | 83.3 |
| Example 17-1 | 3002 | 83.9 |
| Example 17-2 | 2985 | 84.2 |
| Example 18-1 | 2354 | 75.6 |
| Example 18-2 | 2341 | 75.9 |
| Example 19-1 | 2378 | 76.4 |
| Example 19-2 | 2365 | 76.6 |
| Example 20-1 | 2402 | 77.2 |
| Example 20-2 | 2388 | 77.5 |
| Comparative examples 1 to 1 | 2314 | 74.4 |
| Comparative examples 1 to 2 | 2298 | 74.7 |
| Comparative example 2-1 | 2140 | 72.5 |
| Comparative examples 2 to 2 | 2128 | 72.8 |
| Comparative example 3-1 | 2161 | 73.3 |
| Comparative examples 3 to 2 | 2149 | 73.6 |
From the cell cycling and data storage of the comparative and example cells in table 2, it can be seen that the addition of lithium salts to the electrodes of examples 1-20, relative to comparative example 1, can reduce the increase in resistance during cycling of the battery, thereby improving the cycling performance of the battery; in addition, as can be seen from the comparison of the data of examples 1 to 17 and examples 18 and 20, in the case that the content of the lithium salt in the active material sublayer farthest from the current collector is 0 to 2 wt%, which is preferred in the present disclosure, the influence of excessively high viscosity of the electrolyte on the capacity retention rate of the battery during the cycle due to the large dissolution of the upper lithium salt in the electrolyte in the initial state can be avoided, so that the battery can maintain good cycle performance during the cycle.
Test example 3
At room temperature, 2 cells of comparative examples and MOL (initial state of cycle, capacity retention rate of 100%) in examples are charged to 4.2V by using 0.33C constant current and constant voltage respectively, then 1C is used for discharging for 30min to 50% SOC, 4C current is used for discharging for 10S, and voltage values before and after discharging are recorded;
at room temperature, 2 cells of comparative examples and MOL (middle cycle state, capacity retention rate of 90%) in the examples are charged to 4.2V by using a 0.33C constant current and constant voltage, then 1C is used for discharging for 30min to 50% SOC, 4C current is used for discharging for 10S, and voltage values before and after discharging are recorded;
at room temperature, 2 cores of comparative example and example EOL (at the end of cycle, with a capacity retention rate of 80%) are respectively charged to 4.2V by using a 0.33C constant current and a constant voltage, then 1C is used for discharging for 30min to 50% SOC, 4C is used for discharging for 10S, and voltage values before and after discharging are recorded;
discharge dc impedance (voltage before discharge-voltage after discharge)/discharge current; discharge power (pre-discharge voltage-lower limit voltage) lower limit voltage/discharge dc impedance. The results are shown in Table 3.
TABLE 3
Through the direct-current impedance and power data of the cells of the comparative examples and the examples in table 3 in the whole life cycle, it can be seen that the cell impedance and power attenuation of the cells of examples 1-20 in the middle cycle state and the end cycle state are obviously smaller than those of the cells of comparative examples 1-3; the active material layer electrodes of examples 1 to 20 using a plurality of sub-layers containing lithium salt can greatly improve the resistance and power fade in the life cycle, relative to comparative examples 1 to 2; as can be seen from the comparison of the data of examples 1-17 with examples 18 and 20, in the case where the lithium salt content in the active material sub-layer farthest from the current collector is 0-2 wt% as preferred in the present disclosure, the lithium salt in the electrode starts to act as the battery cycle progresses, having an improved effect on the life cycle resistance and power decay.
The preferred embodiments of the present disclosure have been described above in detail, however, the present disclosure is not limited to the specific details of the above embodiments, and various simple modifications may be made to the technical solution of the present disclosure within the technical idea of the present disclosure, and these simple modifications are within the protective scope of the present disclosure.
It should be noted that, in the above embodiments, the various technical features described in the above embodiments may be combined in any suitable manner, and in order to avoid unnecessary repetition, various combinations that may be possible in the present disclosure are not described separately.
In addition, any combination of various embodiments of the present disclosure may be made, and the same should be considered as the disclosure of the present disclosure, as long as it does not depart from the spirit of the present disclosure.
Claims (9)
1. A lithium ion battery, wherein an anode and/or a cathode of the lithium ion battery includes a current collector and an active material layer laminated on a surface of the current collector, the active material layer contains an electrode active material and a first lithium salt, the content of the first lithium salt in the active material layer is not more than 10 wt%, and the active material layer has a concentration gradient in which a concentration of the first lithium salt decreases in a direction away from the current collector;
the active material layer comprises a plurality of active material sub-layers which are stacked, and the concentration of the first lithium salt in the active material sub-layers is gradually decreased along the direction away from the current collector; wherein, in the active material sub-layer farthest from the current collector, the content of the first lithium salt is 0-2 wt%;
the lithium ion battery also comprises a diaphragm and electrolyte.
2. The lithium ion battery of claim 1, wherein the number of the plurality of active material sublayers is 2-6.
3. The lithium ion battery of claim 2, wherein the number of the plurality of active material sublayers is 2; the content of the first lithium salt in the active material sublayer closest to the current collector is 1-5 wt%, and the content of the first lithium salt in the active material sublayer farthest from the current collector is 0-2 wt%.
4. The lithium ion battery of claim 3, wherein the first lithium salt is present in an amount of 2-4 wt% in the active material sublayer closest to the current collector and 0-1 wt% in the active material sublayer furthest from the current collector.
5. The lithium ion battery according to any one of claims 1 to 4, wherein the thickness of the active material layer is 30 to 300 μm; the active material sub-layer has a thickness of 5 to 95% based on the thickness of the active material layer.
6. The lithium ion battery of claim 1, wherein the first lithium salt comprises LiPF 6 、LiClO 4 、LiBO 2 、LiAsF 6 And LiBF 4 One or more of the above; the current collector is selected from aluminum foil and/or copper foil;
the active substance layer of the anode contains an anode active substance, and the anode active substance comprises one or more of natural graphite, artificial graphite, soft carbon, hard carbon and silicon alloy; alternatively, the first and second electrodes may be,
the active material layer of the cathode contains a cathode active material, and the cathode active material comprises LiNi x Co y Mn z O 2 、LiFe a Al b P c O 4 Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is equal to 1; a is more than or equal to 0 and less than or equal to 1, b is more than or equal to 0 and less than or equal to 0.8, c is more than or equal to 0 and less than or equal to 2, and a + b + c is equal to 2.
7. The lithium ion battery of claim 1, wherein the separator is one or more of a polyethylene separator, a polypropylene separator and a non-woven fabric separator;
the electrolyte contains a second solvent and a second lithium salt; the second solvent comprises a cyclic ester and/or a linear ester; the second lithium salt is LiPF 6 、LiClO 4 、LiBO 2 、LiAsF 6 And LiBF 4 One or more of them.
8. The lithium ion battery of claim 7, wherein the second solvent is one or more of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate, and ethyl methyl carbonate.
9. The lithium ion battery of claim 1, wherein the lithium ion battery is a lithium ion power battery.
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